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Dalila Bounoua

Publications and source records attributed to Dalila Bounoua.

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Real-space manifestation of ferroic multipoles in altermagnetic MnF$_2$

Altermagnets are unconventional spin split magnets arising from the zero spin-orbit coupled limit. They host a magnetic multipolar order parameter yet direct real-space observation of these multipoles has remained elusive. Here we use polarized-neutron diffraction to reconstruct the three-dimensional magnetization density of the prototypical altermagnet MnF$_2$. By exploiting symmetry-selective magnetic reflections, we separate the dominant spherical Mn$^{2+}$ contribution from the much weaker anisotropic Mn magnetization and the covalent spin polarization of the fluorine ligands. The reconstructed spin density reveals a finite fluorine ion moment together with an anisotropic Mn magnetization consistent with the symmetry-allowed altermagnetic rank-5 magnetic multipole $O_{52}$(magnetic triacontadipole). These results provide direct real-space evidence of ferroic multipolar order in an altermagnet and establish polarized-neutron diffraction as a powerful probe of hidden magnetic multipoles in quantum materials.

cond-mat.str-el

Orbital current signature using neutron diffraction

We review the hallmarks of orbital loop currents in various correlated electron materials and how they have been evidenced using polarized neutron diffraction. Over the last 20 years, loop current signatures have been observed in high temperature copper oxide superconductors, iridates, copper oxides spin ladders and recently kagome vanadate superconductors. Such currents induce orbital magnetic moments within the unit cell of these quantum materials that can be detected through their interaction with the neutron spin. In addition to the usual description of orbital moments using point-like local magnetic moments, we here show an alternative description of the neutron magnetic cross-section involving the microscopic currents running between different atomic orbitals. We discuss the corresponding magnetic structure factors and the resulting quantitative differences between both approaches.

cond-mat.str-el

Altermagnetism revealed by polarized neutrons in MnF$_2$

Motivated by possible spintronics applications in antiferromagnets, it was recently observed that symmetry admits magnets that combine attractive features of both ferromagnets and antiferromagnets. These systems, dubbed altermagnets, have been the subject of intense study with direct spectroscopic evidence, from ARPES and RIXS, techniques reported in a handful of materials in the last year. Inelastic neutron scattering (INS) is one of the most powerful direct probes of magnetism and has recently been used to witness a splitting of magnon bands in MnTe that is compatible with altermagnetism although the nature and origin of the splitting remain to be fully characterized. However, the full power of neutron scattering for such systems comes from using polarized neutrons to measure the chirality of the magnon bands. Such a measurement provides a direct characterization of altermagnetism directly from the spin wave excitations. In this article, we present results on MnF$_2$ once thought to be an archetypal antiferromagnet. We present a polarized INS data that demonstrate the material is, in fact, altermagnetic. It had long been realized that the magnon bands in this material should have a weak splitting coming from the long-range dipolar coupling. Our data is the first to visualize this splitting directly. While the dipolar splitting on its own is not altermagnetic, using a domain biased sample, the data reveals a nonzero chirality in the neutron scattering cross section that reverses sign between the two magnon modes. It is this feature that clearly demonstrates altermagnetism in MnF$_2$. This finding highlights the potential for polarized INS to characterize altermagnets not least through its exquisite sensitivity to fine-structure in the magnon spectrum.

cond-mat.str-el

Gapped commensurate antiferromagnetic response in a strongly underdoped model cuprate superconductor

It is a distinct possibility that spin fluctuations are the pairing interactions in a wide range of unconventional superconductors. In the case of the high-transition-temperature (high-$T_c$) cuprates, in which superconductivity emerges upon doping an antiferromagnetic Mott-insulating state, spin correlations might furthermore drive unusual pseudogap phenomena. Here we use polarized and unpolarized magnetic neutron scattering to study the simple tetragonal cuprate $\mathrm{HgBa}_{2}\mathrm{CuO}_{4+δ}$ at very low doping ($T_c \approx 55$ K, hole concentration $p \approx 0.064$). In stark contrast to prior results for other underdoped cuprates, we find no evidence of incommensurate spin-density-wave, charge-spin stripe, or $q = 0$ magnetic order. Instead, the antiferromagnetic response in both the superconducting and pseudogap states is gapped below $Δ_\mathrm{AF} \approx 6$ meV, commensurate over a wide energy range, and disperses above about 55 meV. Given the documented model nature of $\mathrm{HgBa}_{2}\mathrm{CuO}_{4+δ}$, which exhibits high structural symmetry and minimal point disorder effects, we conclude that the observed behavior signifies the unmasked response of the quintessential $\mathrm{CuO}_{2}$ planes near the Mott-insulating state. These results for $\mathrm{HgBa}_{2}\mathrm{CuO}_{4+δ}$ can therefore be expected to serve as a benchmark for a refined theoretical understanding of the cuprates.

cond-mat.supr-con

Search for orbital magnetism in the kagome superconductor ${\rm CsV_3Sb_5}$ using neutron diffraction

As many Kagome metals, the topological superconductor AV$_3$Sb$_5$ with (A = K,Rb,Cs) hosts a charge density wave . A related chiral flux phase that breaks the time-reversal symmetry has been further theoretically predicted in these materials. The flux phase is associated with loop currents that produce ordered orbital magnetic moments, which would occur at the momentum points, $\bf M$, characterizing the charge-density wave state. Polarized neutron-diffraction experiments have been performed on an assembly of single crystals of ${\rm CsV_3Sb_5}$ to search for such orbital magnetic moments. No evidence for the existence of a three-dimensionally ordered moment is found at any temperature at the first ${\bf M_1}$=(1/2,0,0) point in the Brillouin zone within an excellent experimental uncertainty, ${\it i.e.}$ ${\bf m}=0 \pm 0.01μ_B$ per vanadium atom. However, a hint to a magnetic orbital moment is found in the second Brillouin zone at {\bf M$_2$}=(1/2,1/2,0) at the detection limit of the experiment. Some loop currents patterns flowing ${\it only}$ on vanadium triangles are able to account for this finding suggesting an ordered orbital magnetic moment of, at most, $\sim 0.02 \pm 0.01μ_B$ per vanadium triangle.

cond-mat.str-el

Universality of the {\bf q}=1/2 Orbital Magnetism in the Pseudogap Phase of the High-$T_c$ superconductor $\rm YBa_{2}Cu_{3}O_{6+x}$

Several decades of debate have centered around the nature of the enigmatic pseudo-gap state in high temperature superconducting copper oxides. Recently, we reported polarized neutron diffraction measurements that suggested the existence of a magnetic texture bound to the pseudo-gap phase [Bounoua, {\it et al}. Communications Physics 5, 268 (2022)]. Such a magnetic texture is likely to involve the spontaneous appearance of loop currents within the CuO$_2$ unit cells, which give birth to complex correlated patterns. In the underdoped ${\rm YBa_{2}Cu_{3}O_{6.6}}$, the magnetic structure factor of such an orbital magnetic texture gives rise to two distinct magnetic responses at {\bf q}=0 and {\bf q}=1/2. As this pattern alters the lattice translation invariance, such a state of matter could contribute to an instability of the Fermi surface. Here, we report polarized neutron scattering measurements on a nearly optimally doped high quality single crystal of ${\rm YBa_{2}Cu_{3}O_{6.9}}$ that exhibits the same {\bf q}=1/2 magnetism and a weakly overdoped ${\rm YBa_{2}Cu_{3}O_{7}}$ sample where this signal is no longer sizeable. The in-plane and out-of-plane magnetic neutron scattering intensities in ${\rm YBa_{2}Cu_{3}O_{6.9}}$ (at {\bf q}=1/2) and ${\rm YBa_{2}Cu_{3}O_{6.85}}$ (at {\bf q}=0), reported previously, display the same temperature dependent hallmarks. The magnitudes of both {\bf q}=0 and {\bf q}=1/2 magnetic signals further exhibit the same trends upon doping in ${\rm YBa_{2}Cu_{3}O_{6+x}}$, confirming that they are likely intertwined.

cond-mat.str-el

Hidden Magnetic Texture in the Pseudogap Phase of High-Tc $YBa_{2}Cu_{3}O_{6.6}$

Despite decades of intense researches, the enigmatic pseudo-gap (PG) phase of superconducting cuprates remains an unsolved mystery. In the last 15 years, various symmetry breakings in the PG state have been discovered, spanning an intra-unit cell (IUC) magnetism, preserving the lattice translational (LT) symmetry but breaking time-reversal symmetry and parity, and an additional incipient charge density wave breaking the LT symmetry upon cooling. However, none of these states can (alone) account for the partial gapping of the Fermi surface. Here we report a hidden LT-breaking magnetism uisng polarized neutron diffraction. Our measurements reveal magnetic correlations, in two different underdoped $\rm YBa_{2}Cu_{3}O_{6.6}$ single crystals, that settle at the PG onset temperature with i) a planar propagation wave vector $(π,0) \equiv (0,π)$, yielding a doubling or quadrupling of the magnetic unit cell and ii) magnetic moments mainly pointing perpendicular to the $CuO_{2}$ layers. The LT-breaking magnetism is at short range suggesting the formation of clusters of 5-6 unit cells. Together with the previously reported IUC magnetism, it yields a hidden magnetic texture of the $CuO_{2}$ unit cells hosting loop currents, forming large supercells which may be crucial for elucidating the PG puzzle.

cond-mat.supr-con

Loop currents in quantum matter

In many quantum materials, strong electron correlations lead to the emergence of new states of matter. In particular, the study in the last decades of the complex phase diagram of high temperature superconducting cuprates highlighted intra-unit-cell electronic instabilities breaking discrete Ising-like symmetries, while preserving the lattice translation invariance. Polarized neutron diffraction experiments have provided compelling evidences supporting a new form of intra-unit-cell magnetism, emerging concomitantly with the so-called pseudogap state of these materials. This observation is currently interpreted as the magnetic hallmark of an intra-unit-cell loop current order, breaking both parity and time-reversal symmetries. More generally, this magneto-electric state is likely to exist in a wider class of quantum materials beyond superconducting cuprates. For instance, it has been already observed in hole-doped Mott insulating iridates or in the spin liquid state of hole-doped 2-leg ladder cuprates.

cond-mat.str-el

Magnetization density distribution of Sr$_2$IrO$_4$: Deviation from a local $j_\text{eff}=1/2$ picture

$5d$ iridium oxides are of huge interest due to the potential for new quantum states driven by strong spin-orbit coupling. The strontium iridate Sr$_2$IrO$_4$ is particularly in the spotlight because of the so-called $j_\text{eff}=1/2$ state consisting of a quantum superposition of the three local $t_{2g}$ orbitals with -- in its most simple version -- nearly equal population, which stabilizes an unconventional Mott insulating state. Here, we report an anisotropic and aspherical magnetization density distribution measured by polarized neutron diffraction in a magnetic field up to 5~T at 4~K, which strongly deviates from a local \jeffHalf picture even when distortion-induced deviations from the equal weights of the orbital populations are taken into account. Once reconstructed by the maximum entropy method and multipole expansion model refinement, the magnetization density shows cross-shaped positive four lobes along the crystallographic tetragonal axes with a large spatial extent, showing that the $xy$ orbital contribution is dominant. The analogy to the superconducting copper oxide systems might then be weaker than commonly thought.

cond-mat.str-el

Loop Currents in Two-leg Ladder Cuprates

New phases with broken discrete Ising symmetries are uncovered in quantum materials with strong electronic correlations. The two-leg ladder cuprate \textbf{$Sr_{14-x}Ca_{x}Cu_{24}O_{41}$} hosts a very rich phase diagram where, upon hole doping, the system exhibits a spin liquid state ending to an intriguing ordered magnetic state at larger $Ca$ content. Using polarized neutron diffraction, we report here the existence of short range magnetism in this material for two $Ca$ contents, whose origin cannot be ascribed to Cu spins. This magnetism develops exclusively within the two-leg ladders with a diffraction pattern at forbidden Bragg scattering which is the hallmark of loop current-like magnetism breaking both time-reversal and parity symmetries. Our discovery shows local discrete symmetry breaking in a one dimensional spin liquid system as theoretically predicted. It further suggests that a loop current-like phase could trigger the long range magnetic order reported at larger doping in two-leg ladder cuprates.

cond-mat.str-el

Evidence for Intra-Unit Cell Magnetism in Superconducting Cuprates: a Technical Assessment

Intra unit cell (IUC) magnetic order observed by polarized neutron diffraction (PND) is one of the hallmarks of the pseudogap state of high-temperature copper oxide superconductors. This experimental observation, usually interpreted as a result of loop currents, has been recently challenged based on lower statistics data. We here address the crucial issue of polarization inhomogeneities in the neutron beams showing that the original data had a much better reproducibilty. Within these technical limitations, we here propose a self-consistent analysis that potentially solves the controversy. We show that all the reported PND experiments in superconducting cuprates are actually compatible with the existence of an IUC magnetism.

cond-mat.supr-con

The effect of different in-chain impurities on the magnetic properties of the spin chain compound SrCuO$_2$ probed by NMR

The S=1/2 Heisenberg spin chain compound SrCuO2 doped with different amounts of nickel (Ni), palladium (Pd), zinc (Zn) and cobalt (Co) has been studied by means of Cu nuclear magnetic resonance (NMR). Replacing only a few of the S=1/2 Cu ions with Ni, Pd, Zn or Co has a major impact on the magnetic properties of the spin chain system. In the case of Ni, Pd and Zn an unusual line broadening in the low temperature NMR spectra reveals the existence of an impurity-induced local alternating magnetization (LAM), while exponentially decaying spin-lattice relaxation rates $T_1^{-1}$ towards low temperatures indicate the opening of spin gaps. A distribution of gap magnitudes is proven by a stretched spin-lattice relaxation and a variation of $T_1^{-1}$ within the broad resonance lines. These observations depend strongly on the impurity concentration and therefore can be understood using the model of finite segments of the spin 1/2 antiferromagnetic Heisenberg chain, i.e. pure chain segmentation due to S = 0 impurities. This is surprising for Ni as it was previously assumed to be a magnetic impurity with S = 1 which is screened by the neighboring copper spins. In order to confirm the S = 0 state of the Ni, we performed x-ray absorption spectroscopy (XAS) and compared the measurements to simulated XAS spectra based on multiplet ligand-field theory. Furthermore, Zn doping leads to much smaller effects on both the NMR spectra and the spin-lattice relaxation rates, indicating that Zn avoids occupying Cu sites. For magnetic Co impurities, $T_1^{-1}$ does not obey the gap like decrease, and the low-temperature spectra get very broad. This could be related to the increase of the Neel temperature which was observed by recent muSR and susceptibility measurements, and is most likely an effect of the impurity spin $S\neq0$.

cond-mat.str-el